IP Library Granted Patent US 8,835,684
Granted Patent B2
US 8,835,684 · App. 12/840,832 · Granted Sep 16, 2014

Preparation of 2R,3S-

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Quick Facts
Patent No.
US 8,835,684
App. No.
12/840,832
Granted
Sep 16, 2014
Kind
B2
Abstract

The present invention provides a new process for the preparation of 2R,3S-N-isobutyl-N-(2-hydroxy-3-amino-4-phenylbutyl)-p-nitrobenzenesulfonylamide hydrochloride, wherein this compound is prepared directly from the chloromethylalcohol. Importantly, the process of the present invention results in higher yields of 2R,3S-N-isobutyl-N-(2-hydroxy-3-amino-4-phenylbutyl)-p-nitrobenzenesulfonylamide hydrochloride without sacrificing its purity. The processes of the present invention can be used to prepare not only the 2R,3S-derivative, but also the 2S,3S-, 2S,2R- and the 2R,3R-derivatives.

Claims (41)

1. A process for preparing a compound having the following general formula:

said process comprising:

(a) combining a halomethyl alcohol (HMA) and an amine in a halogenated solvent with aqueous bicarbonate to form a reaction mixture, and heating said reaction mixture to a temperature ranging from about 10° C. to about 50° C., wherein said HMA has the following general formula:

(b) adding to said first reaction mixture nosyl chloride while stirring said reaction mixture, and recovering the organic layer of said reaction mixture to form a solution; and

(c) reacting said solution with an acid having a pK a of less than about 4 until the reaction is complete, thereby forming the compound of Formula III;

wherein:

R 1 is an amino acid side chain or a functionalized amino acid side chain;

R 2 is a protecting group;

R 3 is a member selected from the group consisting of hydrogen, alkyl, cycloalkyl, aryl and —NHP, wherein P is selected from the group consisting of H, alkyl, cycloalkyl, aryl and a protecting group;

X − is the conjugate base of said acid; and

L is a leaving group.

2. The process in accordance with claim 1 , wherein said amine is a member selected from the group consisting of primary amines, secondary amines, substituted amines, hydrazines and substituted hydrazines.

3. The process in accordance with claim 1 , wherein said amine is a member selected from the group consisting of methylamine, ethylamine, isopropylamine, n-butylamine, isobutylamine, cyclohexylamine, benzylamine, paranitrobenzylamine, dimethylamine, isobutylmethylamine, decahyroquinoline, decahydroisoquinoline, pyrimidine, isobutylhydrazine and t-Boc-hydrazine.

4. The process in accordance with claim 3 , wherein said amine is isobutylamine (IBA).

5. The process in accordance with claim 1 , wherein said halogenated solvent is a member selected from the group consisting of methylene chloride, chloroform, trifluorotoluene (oxsol), parachlorotrifluorotoluene and trichloroethylene.

6. The process in accordance with claim 1 , wherein said halogenated solvent is methylene chloride.

7. The process in accordance with claim 1 , wherein said acid is a member selected from the group consisting of HCl, HBr, CF 3 CO 2 H, CF 3 SO 3 H, CH 3 SO 3 H, H 2 SO 4 , citric acid, tartaric acid, oxalic acid and p-toluene sulfonic acid.

8. The process in accordance with claim 7 , wherein said acid is HCl.

9. The process in accordance with claim 1 , wherein said HMA is a 2S,3S-HMA.

10. The process in accordance with claim 9 , wherein said 2S,3S-HMA has the following general formula:

11. The process in accordance with claim 10 , wherein said compound of Formula III has the following general formula:

12. The process in accordance with claim 1 , wherein said reaction mixture is heated to a temperature ranging from about 30° C. to about 35° C.

13. A process for preparing a compound having the following general formula:

said process comprising:

(a) adding a compound of Formula I in a halogenated solvent with a tertiary amine and nosyl chloride to form a reaction mixture, and heating said reaction mixture at a temperature ranging from about 10° C. to about 50° C., said compound of Formula I having the following general formula:

(b) reacting said reaction mixture with an acid having a pK a of less than about 4 until the reaction is complete, thereby forming the compound of Formula III;

wherein:

R 1 is an amino acid side chain or a functionalized amino acid side chain;

R 2 is a reacting group;

R 3 and R 4 are independently selected from the group consisting of hydrogen, alkyl, cycloalkyl, aryl and —NHP, wherein P is selected from the group consisting of H, alkyl, cycloalkyl, aryl and a protecting group, or R 3 and R 4 together form a cyclic structure selected from the group consisting of quinoline and isoquinoline; and

X − is the conjugate base of said acid.

14. The process in accordance with claim 13 , wherein said compound of Formula I has the following general formula:

15. The process in accordance with claim 14 , wherein said compound of Formula III has the following general formula:

16. The process in accordance with claim 13 , wherein said halogenated solvent is a member selected from the group consisting of methylene chloride, chloroform, trifluorotoluene (oxsol), parachlorotrifluorotoluene and trichloroethylene.

17. The process in accordance with claim 13 , wherein said halogenated solvent is methylene chloride.

18. The process in accordance with claim 13 , wherein said acid is a member selected from the group consisting of HCl, HBr, CF 3 CO 2 H, CF 3 SO 3 H, CH 3 SO 3 H, H 2 SO 4 , citric acid, tartaric acid, oxalic acid and p-toluene sulfonic acid.

19. The process in accordance with claim 18 , wherein said acid is HCl.

20. The process in accordance with claim 13 , further comprising washing, heating and azeotropically drying said reaction mixture prior to step (b).

21. The process in accordance with claim 13 , further comprising:

(c) recovering said compound of Formula III from said reaction mixture.

22. The process in accordance with claim 13 , wherein said reaction mixture is heated to a temperature ranging from about 30° C. to about 35° C.

Assignments (9)
CORRECTIVE ASSIGNMENT TO CORRECT THE INCORRECT STATEMENT THAT THIS DOCUMENT SERVES AS AN OATH/DECLARATION PREVIOUSLY RECORDED AT REEL: 047383 FRAME: 0438. ASSIGNOR(S) HEREBY CONFIRMS THE TERMINATION AND RELEASE OF SECURITY INTEREST IN PATENTS. Recorded Nov 5, 2018
From: KEYBANK NATIONAL ASSOCIATION, AS COLLATERAL AGENT
To: AMPAC FINE CHEMICALS LLC
Reel/Frame 047422/0852 →
TERMINATION AND RELEASE OF SECURITY INTEREST IN PATENTS Recorded Aug 31, 2018
From: KEYBANK NATIONAL ASSOCIATION, AS COLLATERAL AGENT
To: AMPAC FINE CHEMICALS LLC
Reel/Frame 047383/0437 →
GRANT OF SECURITY INTEREST IN PATENTS Recorded Aug 3, 2018
From: AMPAC FINE CHEMICALS LLC
To: KEYBANK NATIONAL ASSOCIATION
Reel/Frame 046703/0605 →
RELEASE OF SECURITY INTEREST IN PATENTS RECORDED AT R/F: 032365/0398 Recorded Dec 15, 2015
From: JEFFERIES FINANCE LLC, AS ADMINISTRATIVE AGENT
To: AMPAC FINE CHEMICALS LLC
Reel/Frame 037300/0399 →
PATENT RELEASE AND REASSIGNMENT (R/F 029370/0835) Recorded Feb 27, 2014
From: KEYBANK NATIONAL ASSOCIATION, AS AGENT
To: AMPAC FINE CHEMICALS LLC
Reel/Frame 032363/0222 →
SECURITY AGREEMENT Recorded Feb 27, 2014
From: AMPAC FINE CHEMICALS LLC
To: JEFFERIES FINANCE LLC, AS ADMINISTRATIVE AGENT
Reel/Frame 032365/0398 →
COLLATERAL ASSIGNMENT AND SECURITY INTEREST OF PATENTS Recorded Nov 28, 2012
From: AMPAC FINE CHEMICALS LLC
To: KEYBANK NATIONAL ASSOCIATION
Reel/Frame 029370/0835 →
CORRECTIVE ASSIGNMENT TO CORRECT THE ASSIGNEE FROM AMERICAN FINE CHEMICALS LLC TO AMPAC FINE CHEMICALS LLC PREVIOUSLY RECORDED ON REEL 029203 FRAME 0091. ASSIGNOR(S) HEREBY CONFIRMS THE RELEASE BY SECURED PARTY. Recorded Nov 5, 2012
From: WELLS FARGO BANK, NATIONAL ASSOCIATION
To: AMPAC FINE CHEMICALS LLC
Reel/Frame 029245/0597 →
RELEASE OF SECURITY INTEREST Recorded Oct 26, 2012
From: WELLS FARGO BANK, NATIONAL ASSOCIATION
To: AMERICAN FINE CHEMICALS LLC
Reel/Frame 029203/0091 →